The photocatalysts of Fe-ACF/TiO2 compositeswere prepared by the sol-gel method and characterizedby BET, XRD, SEM, and EDX. It showed that the BET surface area was related to adsorption capacity foreach composite. The SEM results showed that ferric compound and titanium dioxide were distributed on thesurfaces of ACF. The XRD results showed that Fe-ACF/TiO2 composite only contained an anatase structurewith a Fe mediated compound. EDX results showed the presence of C, O, and Ti with Fe peaks in Fe-ACF/TiO2 composites. From the photocataytic degradation effect, TiO2 on activated carbon fiber surface modifiedwith Fe (Fe-ACF/TiO2) could work in the photo-Fenton process. It was revealed that the photo-Fenton reactiongives considerable photocatalytic ability for the decomposition of methylene blue (MB) compared to non-treatedACF/TiO2, and the photo-Fenton reaction was improved by the addition of H2O2. It was proved that thedecomposition of MB under UV (365nm) irradiation in the presence of H2O2 predominantly accelerated theoxidation of Fe2+ to Fe3+ and produced a high concentration of OH. radicals.